An abiotic analogue of methane monooxygenase for the catalytic oxidation of hydrocarbons in homogeneous conditions

DOI

We propose to use INS to characterise the structural and vibrational properties of a new class of Fenton-like Fe(IV)O intermediates of potential relevance in the conversion of methane into methanol in homogeneous catalytic conditions for fuel production. On the basis of extensive DFT and ab initio molecular dynamics simulations, we have established that Fe(IV)O/EDTA species with remarkable catalytic activity can be generated from the direct reduction of atmospheric dioxygen by Fe(II)/EDTA in water solution. The reduction occurs through a complex mechanism which bears strong resemblance to the catalytic cycle of methane monooxygenase, an enzyme responsible for methane-to-methanol conversion in some classes of extremophiles. We will compare experimental data with DFT calculations to establish a link between the EDTA/Fe(IV)O chelation geometry and the catalytic properties of the compound.

Identifier
DOI https://doi.org/10.5286/ISIS.E.73943993
Metadata Access https://icatisis.esc.rl.ac.uk/oaipmh/request?verb=GetRecord&metadataPrefix=oai_datacite&identifier=oai:icatisis.esc.rl.ac.uk:inv/73943993
Provenance
Creator Professor Stewart Parker; Dr Leonardo Bernasconi; Dr Svemir Rudic
Publisher ISIS Neutron and Muon Source
Publication Year 2019
Rights CC-BY Attribution 4.0 International; https://creativecommons.org/licenses/by/4.0/
OpenAccess true
Contact isisdata(at)stfc.ac.uk
Representation
Resource Type Dataset
Discipline Chemistry; Natural Sciences
Temporal Coverage Begin 2016-02-25T09:00:00Z
Temporal Coverage End 2016-02-28T09:00:00Z